Show simple item record

dc.contributor.authorDong, Chunwei
dc.contributor.authorHuang, Renwu
dc.contributor.authorChen, Cailing
dc.contributor.authorChen, Jie
dc.contributor.authorNematulloev, Saidkhodzha
dc.contributor.authorGuo, Xianrong
dc.contributor.authorGhosh, Atanu
dc.contributor.authorAlamer, Badriah Jaber
dc.contributor.authorHedhili, Mohamed N.
dc.contributor.authorIsimjan, Tayirjan T.
dc.contributor.authorHan, Yu
dc.contributor.authorMohammed, Omar F.
dc.contributor.authorBakr, Osman
dc.date.accessioned2021-07-14T06:32:05Z
dc.date.available2021-07-14T06:32:05Z
dc.date.issued2021-07-13
dc.date.submitted2021-04-06
dc.identifier.citationDong, C., Huang, R.-W., Chen, C., Chen, J., Nematulloev, S., Guo, X., … Bakr, O. M. (2021). [Cu36H10(PET)24(PPh3)6Cl2] Reveals Surface Vacancy Defects in Ligand-Stabilized Metal Nanoclusters. Journal of the American Chemical Society. doi:10.1021/jacs.1c03402
dc.identifier.issn0002-7863
dc.identifier.issn1520-5126
dc.identifier.doi10.1021/jacs.1c03402
dc.identifier.urihttp://hdl.handle.net/10754/670195
dc.description.abstractPrecise identification and in-depth understanding of defects in nanomaterials can aid in rationally modulating defect-induced functionalities. However, few studies have explored vacancy defects in ligand-stabilized metal nanoclusters with well-defined structures, owing to the substantial challenge of synthesizing and isolating such defective metal nanoclusters. Herein, a novel defective copper hydride nanocluster, [Cu36H10(PET)24(PPh3)6Cl2] (Cu36; PET: phenylethanethiolate; PPh3: triphenylphosphine), is successfully synthesized at the gram scale via a simple one-pot reduction method. Structural analysis reveals that Cu36 is a distorted half cubic nanocluster, evolved from the perfect Nichol’s half cube. The two surface copper vacancies in Cu36 are found to be the principal imperfections, which result in some structural adjustments, including copper atom reconstruction near the vacancies as well as ligand modifications (e.g., substitution, migration, and exfoliation). Density functional theory calculations imply that the above-mentioned defects have a considerable influence on the electronic structure and properties. The modeling suggests that the formation of defective Cu36 rather than the perfect half cube is driven by the enlargement of the energy gap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital of the nanocluster. The structural evolution induced by the surface copper atom vacancies provides atomically precise insights into the defect-induced readjustment of the local structure and introduces new avenues for understanding the chemistry of defects in nanomaterials.
dc.description.sponsorshipThis work was supported by King Abdullah University of Science and Technology (KAUST) and SABIC (grant # RGC/3/3517-01-01).
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttps://pubs.acs.org/doi/10.1021/jacs.1c03402
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.1c03402.
dc.title[Cu36H10(PET)24(PPh3)6Cl2] Reveals Surface Vacancy Defects in Ligand-Stabilized Metal Nanoclusters
dc.typeArticle
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Center
dc.contributor.departmentChemical Science
dc.contributor.departmentNMR
dc.contributor.departmentChemical Science Program
dc.contributor.departmentSurface Science
dc.contributor.departmentKAUST Solar Center (KSC)
dc.contributor.departmentMaterial Science and Engineering Program
dc.identifier.journalJournal of the American Chemical Society
dc.rights.embargodate2022-07-13
dc.eprint.versionPost-print
dc.contributor.institutionSchool of Chemical Engineering and Technology, Xi’an Jiaotong University, Xi’an 710049, China
kaust.personDong, Chunwei
kaust.personHuang, Renwu
kaust.personChen, Cailing
kaust.personNematulloev, Saidkhodzha
kaust.personGuo, Xianrong
kaust.personGhosh, Atanu
kaust.personAlamer, Badriah Jaber
kaust.personHedhili, Mohamed N.
kaust.personIsimjan, Tayirjan T.
kaust.personHan, Yu
kaust.personMohammed, Omar F.
kaust.personBakr, Osman M.
refterms.dateFOA2021-07-15T05:34:01Z


Files in this item

Thumbnail
Name:
Manuscript_Non-highlighted.pdf
Size:
646.2Kb
Format:
PDF
Description:
Accepted manuscript
Embargo End Date:
2022-07-13
Thumbnail
Name:
Supporting Information_Non-highlighted.pdf
Size:
2.192Mb
Format:
PDF
Description:
supporting Information
Embargo End Date:
2022-07-13

This item appears in the following Collection(s)

Show simple item record